WO2015065127A1 - Ensemble électrode à pliage d'empilement - Google Patents

Ensemble électrode à pliage d'empilement Download PDF

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Publication number
WO2015065127A1
WO2015065127A1 PCT/KR2014/010399 KR2014010399W WO2015065127A1 WO 2015065127 A1 WO2015065127 A1 WO 2015065127A1 KR 2014010399 W KR2014010399 W KR 2014010399W WO 2015065127 A1 WO2015065127 A1 WO 2015065127A1
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Prior art keywords
separator
binder
electrode assembly
stack
foldable
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PCT/KR2014/010399
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English (en)
Korean (ko)
Inventor
박지혜
이재헌
이수림
오송택
최정석
이혁무
Original Assignee
주식회사 엘지화학
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Application filed by 주식회사 엘지화학 filed Critical 주식회사 엘지화학
Priority to US14/762,409 priority Critical patent/US9484593B2/en
Priority to CN201480037483.0A priority patent/CN105393399B/zh
Publication of WO2015065127A1 publication Critical patent/WO2015065127A1/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0583—Construction or manufacture of accumulators with folded construction elements except wound ones, i.e. folded positive or negative electrodes or separators, e.g. with "Z"-shaped electrodes or separators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/04—Construction or manufacture in general
    • H01M10/0436—Small-sized flat cells or batteries for portable equipment
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/04—Construction or manufacture in general
    • H01M10/0459—Cells or batteries with folded separator between plate-like electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H01M4/622—Binders being polymers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H01M4/622—Binders being polymers
    • H01M4/623—Binders being polymers fluorinated polymers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
    • H01M50/103—Primary casings; Jackets or wrappings characterised by their shape or physical structure prismatic or rectangular
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/431—Inorganic material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/446—Composite material consisting of a mixture of organic and inorganic materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/449—Separators, membranes or diaphragms characterised by the material having a layered structure
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/449—Separators, membranes or diaphragms characterised by the material having a layered structure
    • H01M50/451—Separators, membranes or diaphragms characterised by the material having a layered structure comprising layers of only organic material and layers containing inorganic material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
    • H01M50/461—Separators, membranes or diaphragms characterised by their combination with electrodes with adhesive layers between electrodes and separators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2220/00—Batteries for particular applications
    • H01M2220/30—Batteries in portable systems, e.g. mobile phone, laptop
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/60—Other road transportation technologies with climate change mitigation effect
    • Y02T10/70—Energy storage systems for electromobility, e.g. batteries

Definitions

  • the present invention relates to a stack-foldable electrode assembly. More particularly, the present invention relates to a stack-foldable electrode assembly having improved battery performance of an electrochemical device.
  • the electrochemical device is the field that is attracting the most attention in this respect, in particular, in accordance with the recent trend of miniaturization and weight reduction of electronic devices, the development of secondary batteries as a battery capable of charging and discharging small size and high capacity has been the focus of attention.
  • secondary batteries are classified according to what kind of structure the electrode assembly has a positive electrode / separator / cathode structure.
  • a long sheet-shaped positive electrode and negative electrode are wound in a state where a separator is interposed.
  • -Roll (electrode) electrode assembly a plurality of positive electrode and negative electrode cut in a predetermined size unit is divided into a stacked (stacked) electrode assembly sequentially stacked with a separator.
  • the jelly-roll electrode assembly is wound around the long sheet-like anode and cathode in a dense state to form a cylindrical or oval structure in cross section, stress caused by expansion and contraction of the electrode during charge and discharge accumulates inside the electrode assembly. If the stress accumulation exceeds a certain limit, deformation of the electrode assembly occurs. Deformation of the electrode assembly causes a problem that the spacing between the electrodes is uneven, so that the performance of the battery is drastically degraded and the safety of the battery is threatened due to an internal short circuit. In addition, since the long sheet-type positive electrode and the negative electrode must be wound, it is difficult to quickly wind the coil while keeping the distance between the positive electrode and the negative electrode, which also has a problem in that the productivity is lowered.
  • the stack type electrode assembly has to stack a plurality of positive and negative electrode units in sequence, a separate electrode plate transfer process is required separately for manufacturing the unit, and a sequential lamination process requires a lot of time and effort, resulting in low productivity. Has a problem.
  • the electrode assembly of the advanced structure in the mixed form of the jelly-roll type and the stack type, a bi-cell or a full cell in which the positive electrode and the negative electrode of a predetermined unit is laminated in the state of the intermediary The stack-folding electrode assembly of a structure in which (Full cells) are wound using a long length of continuous cerapater sheet has been developed, which is disclosed in Korean Patent Application Publication Nos. 2001-0082058, 2001-0082059, and No. 2001-0082060 and the like.
  • FIGS. 1 to 3 are cross-sectional views schematically illustrating a structure of a stack-foldable electrode assembly.
  • like numerals mean like members.
  • the electrode assemblies 10, 20, and 30 may include the cathodes 1a, 1b, which are positioned at both sides of the first separators 3a, 3b, and 3c and the first separators 3a, 3b, and 3c. And a plurality of unit cells 7a, 7b, 7c 1 , 7c 2 each having 1c and positive electrodes 5a, 5b, 5c.
  • the positive electrodes 5a, 5b and 5c have a structure in which positive electrode active material layers are formed on both surfaces of the positive electrode current collector, and the negative electrodes 1a, 1b and 1c have a structure in which negative electrode active material layers are formed on both sides of the negative electrode current collector. As shown in FIGS.
  • the unit cell has a structure of full cells 7a and 7b in which one positive electrode 5a and 5b and one negative electrode 1a and 1b are positioned at both sides of the first separators 3a and 3b.
  • the first separator 3c is positioned on both sides of the positive electrode 5c or the negative electrode 1c, and the bicells 7c 1 in which the negative electrode 1c or the positive electrode 5c are positioned on each of the first separators 3c, respectively.
  • 7c 2 may be formed of unit cells having various structures, such as the structure of the anode / separator / cathode / separator / anode or the structure of the cathode / separator / anode / separator / cathode.
  • each unit cell 7a, 7b, 7c 1 , 7c 2 is present in stacked form.
  • the second separators 9a, 9b, and 9c of Hg are interposed in various forms as shown in FIGS. 1 to 3 to perform a separator function between the unit cells 7a, 7b, 7c 1 , and 7c 2 .
  • the prepared stack-folding electrode assembly is accommodated in a battery case and then injected with an electrolyte to manufacture a battery.
  • the gas generated due to decomposition of the electrolyte and side reaction of the battery causes the inside of the battery to be lifted up, thereby degrading the performance of the battery. That is, it is difficult to suppress the expansion of the battery, thereby degrading the battery performance and when the external impact is vulnerable to deformation may reduce the strength of the battery. In particular, there is a high possibility that such problems may occur in high temperature use.
  • an object of the present invention is to provide a stack-foldable electrode assembly which suppresses the floating phenomenon of the inside of the battery, reduces the expansion of the battery, and reduces the deformation in the external impact.
  • a plurality of unit cells are wrapped around a unit cell of a full cell or bicell including a positive electrode, a negative electrode, and a first separator interposed between the positive electrode and the negative electrode with a second separator.
  • An overlapped stack-foldable electrode assembly wherein the first separator has a first binder coated on at least a portion of the first separator, and the second separator has a second binder coated on at least a portion of the surface of the second separator.
  • the content of the second binder provides a stack-foldable electrode assembly, characterized in that more than the content of the first binder.
  • the content of the second binder may be included 2% to 10% more than the content of the first binder.
  • the first binder and the second binder are independently, polyvinylidene fluoride-co-hexafluoropropylene, polyvinylidene pullo Polyvinylidene fluoride-cotrichloroethylene, polymethylmethacrylate, polyacrylonitrile, polyvinylpyrrolidone, polyvinyacetate, ethylene vinyl acetate copolymer (polyethylene-co-vinyl acetate), polyethylene oxide, cellulose acetate, cellulose acetate butyrate, celluloseacetate propionate, cyanoethylpullulan ), Cyanoethyl polyvinyl alcohol (cyanoethylpol yvinylalcohol, cyanoethylcellulose, cyanoethylsucrose, pullulan, carboxyl methyl cellulose, acrylonitrile-styrene-butadiene copolymer And it may be any one or more selected from the group
  • the first separator and the second separator each independently include a) a porous substrate having pores, or b) a porous substrate having pores and at least one of the porous substrate. It may have a form including an organic-inorganic porous coating layer formed on a surface of a mixture of inorganic particles and a binder polymer.
  • the porous substrate is polyolefin, polyethylene terephthalate, polybutylene terephthalate, polyacetal, polyamide, polycarbonate, polyimide, polyetheretherketone, polyethersulfone, poly It may be formed of at least one selected from the group consisting of phenylene oxide, polyphenylene sulfide and polyethylene naphthalene.
  • Another aspect according to the present invention provides an electrochemical device in which a stack-foldable electrode assembly according to the present invention is housed in a case.
  • the electrochemical device may be a lithium secondary battery.
  • the stack-foldable electrode assembly of the present invention allows the amount of the binder included in the second separator surrounding the unit cells to be added more than the content of the binder included in the first separator, thereby further improving the adhesion of the separator surrounding the unit cells. I was. Through this, the lifting of the inside of the battery generated by the gas generated by the side reaction during the driving of the battery can be suppressed, thereby preventing the performance of the battery from being lowered. In addition, due to the lifting phenomenon inside the battery, it is possible to improve the problem that the deformation is weak when an impact is applied from the outside.
  • FIG. 1 is a schematic cross-sectional view of one embodiment of a stack-foldable electrode assembly.
  • FIG. 2 is a schematic cross-sectional view of another embodiment of a stack-foldable electrode assembly.
  • FIG 3 is a schematic cross-sectional view of another embodiment of a stack-foldable electrode assembly.
  • FIG. 4 is a schematic cross-sectional view of a stack-foldable electrode assembly with unit cells in accordance with one embodiment of the present invention.
  • FIG. 5 is a schematic cross-sectional view of a stack-foldable electrode assembly with bicells in accordance with another embodiment of the present invention.
  • 110, 120, 130, 140, 150 full cell
  • 210, 220, 230, 240, 250 bicell
  • the present invention provides a stack-folding electrode assembly in which a plurality of unit cells are overlapped by enclosing a unit cell of a full cell or bicell including a positive electrode, a negative electrode, and a first separator interposed between the positive electrode and the negative electrode with a second separator.
  • a first separator a first binder is coated on at least a portion of the surface of the first separator, and in the second separator, a second binder is coated on at least a portion of the surface of the second separator, and the content of the second binder is first.
  • Stacked-foldable electrode assembly characterized in that it contains more than the content of the binder.
  • the first separator is a separator existing in the unit cell and is interposed between the anode and the cathode of the unit cell, and the second separator serves to wrap the unit cells differently from the first separator.
  • the adhesive force is high because the first separator is laminated with the electrode, but the adhesive force is not high because the second separator does not undergo a separate lamination. That is, when the second separator is used in the same configuration as the first separator, the second separator, which serves to surround the unit cells, has a lower adhesive force.
  • the inventors of the present invention suggest that, if the surface adhesion of the second separator surrounding the unit cells is further improved, more specifically, the surface adhesion of the second separator surrounding the unit cells may be used to surround the unit cell. If improved than the surface adhesion when used, the present invention was completed by focusing on minimizing the lifting phenomenon caused by the inside of the battery.
  • the content of the second binder further comprises 2% to 10%, preferably 3% to 5% more than the content of the first binder.
  • the surface adhesion of the second separator surrounding the unit cells may be more improved, and more specifically, the surface adhesion force when the first separator is used to surround the unit cells may be improved.
  • the surface adhesion of the second separator may be 3 to 10 gf / cm, and the surface adhesion when the first separator is used to surround the unit cells may be 1 to 2 gf / cm. This surface adhesion is measured by the peel test method.
  • the first binder and the second binder are independently polyvinylidene fluoride-co-hexafluoropropylene (polyvinylidene fluoride-co-hexafluoropropylene), polyvinylidene fluoride-cotrichloroethylene, Polymethylmethacrylate, polyacrylonitrile, polyvinylpyrrolidone, polyvinylacetate, ethylene vinyl acetate copolymer, polyethylene oxide ( polyethylene oxide, cellulose acetate, cellulose acetate butyrate, celluloseacetate propionate, cyanoethylpullulan, cyanoethylpolyvinylalcohol, Cyanoethylcellulose ), Cyanoethylsucrose, pullulan, carboxyl methyl cellulose, acrylonitrile-styrene-butadiene copolymer and polyimide It may be any one or more selected from, and the first binder and the second binder may be the same or
  • the first separator and the second separator according to the present invention may include the first binder and the second binder in the following manner, but are not limited thereto.
  • a binder resin such as polyvinylidene fluoride-chlorotrifluoroethylene copolymer may be acetone, dimethylacetamide (DMA) or N-methyl-2-pyrrolidone (N).
  • DMA dimethylacetamide
  • NMP N-methyl-2-pyrrolidone
  • the surface of the first separator and the second separator is coated. The coating is performed by dip coating, die coating, or roll coating.
  • Another method is to prepare a film from a polymer binder resin such as polyvinylidene fluoride-chlorotrifluoroethylene copolymer, and to prepare the film by laminating and thermally bonding the prepared film on the surface of the first separator and the second separator. It is possible.
  • a polymer binder resin such as polyvinylidene fluoride-chlorotrifluoroethylene copolymer
  • One specific example is to prepare a solution of the polyvinylidene fluoride-chlorotrifluoroethylene copolymer with the solvent described above, and then first to a polyester-based support film such as Mylar or a release paper. After coating and drying to form a film, the film is prepared by a heat lamination process on the surface of the first separator and the second separator.
  • a solvent is not used, and a binder resin such as a polyvinylidene fluoride-chlorotrifluoroethylene copolymer is directly added to an extruder and extruded through a film die to prepare a film, and then a film It is prepared by a heat lamination process (heat lamination process) on the polymer membrane or separation film.
  • the adhesive may be attached to the first separator and the second separator while manufacturing the binder film in an extruder.
  • the first separator and the second separator are each independently a) a porous substrate having pores or b) a porous substrate having pores and a mixture of inorganic particles and a binder polymer on at least one side of the porous substrate. It may be in a form including an organic-inorganic porous coating layer formed.
  • the binder polymer included in the organic-inorganic porous coating layer of the second separator is included in the organic-inorganic porous coating layer of the first separator. More than the polymer, it may mean that the surface adhesion of the second separator is higher than the surface adhesion of the first separator.
  • the porous substrate is polyolefin, polyethylene terephthalate, polybutylene terephthalate, polyacetal, polyamide, polycarbonate, polyimide, polyetheretherketone, polyethersulfone, polyphenylene oxide, polyphenylene sulfide and polyethylene naphthalene It may be formed of at least one selected from the group consisting of, the polyolefin may be any one polymer selected from the group consisting of polyethylene, polypropylene, polybutylene and polypentene.
  • the separator may be composed of a layer structure made of the polymers such as polypropylene / polyethylene / polypropylene.
  • the organic-inorganic porous coating layer is attached to each other (that is, the binder polymer is connected and fixed between the inorganic particles) so that the binder polymer can remain in the state in which the inorganic particles are bound to each other, and the organic-inorganic porous coating layer is attached to the binder polymer Thereby to remain bound to the porous substrate.
  • Inorganic particles of the organic-inorganic porous coating layer are present in the closest packed structure substantially in contact with each other, the interstitial volume generated when the inorganic particles are in contact with the pores of the organic-inorganic porous coating layer.
  • the separator on which the organic-inorganic porous coating layer is formed is excellent in heat resistance, but stability is enhanced, but electrical resistance may increase due to the binder polymer.
  • the inorganic particles are not particularly limited as long as they are electrochemically stable. That is, the inorganic particles that can be used in the present invention are not particularly limited as long as the oxidation and / or reduction reactions do not occur in the operating voltage range (for example, 0 to 5 V on the basis of Li / Li + ) of the applied electrochemical device. In particular, in the case of using the inorganic particles having the ion transport ability, it is possible to improve the performance by increasing the ion conductivity in the electrochemical device.
  • the inorganic particles when inorganic particles having a high dielectric constant are used as the inorganic particles, the ionic conductivity of the electrolyte may be improved by contributing to an increase in the dissociation degree of the electrolyte salt such as lithium salt in the liquid electrolyte.
  • the inorganic particles preferably include high dielectric constant inorganic particles having a dielectric constant of 5 or more, preferably 10 or more, inorganic particles having a lithium ion transfer ability, or a mixture thereof.
  • the thickness of the first separator may be 12 to 16 ⁇ m, and the thickness of the second separator may be 13 to 17 ⁇ m.
  • a typical full cell structure has a structure in which the anode, the cathode, and the layered tissue of the first separator are cut into regular shapes and sizes and then stacked. In this case, all electrodes are coated with an electrode active material based on a current collector. This structure is treated as one unit cell for constituting the battery by lamination, and for this purpose, the electrode and the first separator must adhere the films to each other.
  • a full cell having the structure described above is a structure in which electrodes at both ends, such as an anode / separator / cathode or an anode / separator / cathode / separator / anode / separator / cathode, are formed to form an anode and a cathode, respectively.
  • the bicell has a structure in which electrodes at both ends are stacked to form the same electrode, and a cathode-type bicell composed of anode / separator / cathode / separator / anode and cathode / separator / anode / separator / cathode It is divided into bipolar bicell consisting of.
  • the electrode according to the present invention is not particularly limited and may be prepared by applying an electrode active material slurry to a current collector according to conventional methods known in the art.
  • the positive electrode active material and the negative electrode active material used for the electrode conventional electrode active materials that can be used for the positive electrode and the negative electrode of the conventional electrochemical device may be used.
  • the positive electrode active material of the electrode active material it is preferable to use lithium manganese oxide, lithium cobalt oxide, lithium nickel oxide, lithium iron oxide or a lithium composite oxide in combination thereof.
  • Non-limiting examples of negative electrode active materials include lithium metal or lithium alloys, soft carbon, hard carbon, natural graphite, Kish graphite, pyrolytic carbon, liquid crystal pitch carbon fiber (mesophase pitch based carbon fiber), meso-carbon microbeads, mesophase pitches, petroleum or coal tar pitch derived cokes and the like are preferable.
  • the electrode active material may be added to an organic solvent together with additives such as a binder and a conductive material according to a conventional method in the art to prepare an electrode mixture slurry, and then coated on each electrode current collector to prepare an electrode.
  • additives such as a binder and a conductive material according to a conventional method in the art to prepare an electrode mixture slurry, and then coated on each electrode current collector to prepare an electrode.
  • the positive electrode current collector aluminum, nickel, and the like may be used, and as a non-limiting example of the negative electrode current collector, copper, gold, nickel, or a copper alloy may be used.
  • an electrode assembly may be manufactured using a stack-folding method. Specifically, the second separator is folded in a direction surrounding the unit cell or the bicell, but folded to have a structure in which the unit cells or the bicell are aligned to correspond to each other in a stacked form.
  • the electrodes 101 and 201 located at the top of the unit cell 110 or the bicell 210 can contact the separators 109 and 209 if the folding starts from the right end.
  • all the unit cells 110, 120, 130, 140, and 150 or the bicells 210, 220, 230, 240, and 250 are second separators.
  • the second separators 109 and 209 may be interposed between adjacent unit cells or bicells, and the unit cells or bicells may be stacked and aligned to correspond to each other. You will have (stack-folding). However, in order to perform the stack-folding process as described above, the unit cells 120, 130, 140, 150, and bicells after the first unit cell 110 and the bicell 210 illustrated in FIGS. 4 and 5 are performed.
  • the spacing between the fields 220, 230, 240, and 250 corresponds to the heights of the cells stacked up to each unit cell or bicell, and thus should be gradually widened.
  • the representations are shown at uniform intervals for ease of representation.
  • the lithium salt that may be included as an electrolyte may be used, without limitation, those which are commonly used in a lithium secondary battery electrolyte, such as the lithium salt, the anion is F -, Cl -, Br - , I -, NO 3 -, N (CN) 2-, BF 4 -, ClO 4 -, PF 6 -, (CF 3) 2 PF 4 -, (CF 3) 3 PF 3 -, (CF 3) 4 PF 2 -, (CF 3) 5 PF -, (CF 3) 6 P -, CF 3 SO 3 -, CF 3 CF 2 SO 3 -, (CF 3 SO 2) 2 N -, (FSO 2) 2 N -, CF 3 CF 2 (CF 3) 2 CO -, (CF 3 SO 2) 2 CH -, (SF 5) 3 C -, (CF 3 SO 2) 3 C -, CF 3 (CF 2) 7 SO 3 -, CF 3 CO 2
  • organic solvent included in the electrolyte solution those conventionally used in the electrolyte for lithium secondary batteries may be used without limitation, and typically, propylene carbonate (PC), ethylene carbonate (ethylene carbonate, EC), diethyl carbonate (DEC), dimethyl carbonate (DMC), ethylmethyl carbonate (EMC), methylpropyl carbonate, dipropyl carbonate, dimethylsulfuroxide, acetonitrile, dimethoxyethane, diethoxy Ethylene, vinylene carbonate, sulfolane, gamma-butyrolactone, propylene sulfite, tetrahydrofuran, any one selected from the group consisting of, or a mixture of two or more thereof may be representatively used.
  • PC propylene carbonate
  • EC ethylene carbonate
  • DEC diethyl carbonate
  • DMC dimethyl carbonate
  • EMC ethylmethyl carbonate
  • methylpropyl carbonate dipropy
  • ethylene carbonate and propylene carbonate which are cyclic carbonates among the carbonate-based organic solvents, are highly viscous organic solvents, and thus may be preferably used because they dissociate lithium salts in electrolytes well.
  • Dimethyl carbonate and diethyl When a low viscosity, low dielectric constant linear carbonate, such as carbonate, is mixed and used in an appropriate ratio, an electrolyte having high electrical conductivity can be prepared, and thus it can be more preferably used.
  • the electrolyte solution stored according to the present invention may further include additives such as an overcharge inhibitor included in a conventional electrolyte solution.
  • the battery case used in the present invention may be adopted that is commonly used in the art, there is no limitation on the appearance according to the use of the battery, for example, cylindrical, square, pouch type or coin using a can (coin) type and the like.
  • the electrochemical device When the electrode assembly is completed, the electrochemical device may be manufactured by accommodating and sealing the case in a conventional manner.
  • the electrochemical device is preferably a lithium secondary battery.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Inorganic Chemistry (AREA)
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Abstract

La présente invention concerne un ensemble électrode à pliage d'empilement qui comprend une anode, une cathode, et un premier séparateur interposé entre l'anode et la cathode, et qui chevauche une pluralité de cellules unitaires en enfermant des cellules unitaires à cellule pleine ou à mi-cellule en utilisant un second séparateur. L'ensemble électrode à pliage d'empilement est caractérisé en ce qu'un premier liant est déposé sur au moins une partie d'une surface du premier séparateur, qu'un second liant est déposé sur au moins une partie d'une surface du second séparateur, et que la teneur en second liant est supérieure à la teneur en premier liant. Un ensemble électrode à pliage d'empilement peut être proposé grâce auquel la création d'espaces à l'intérieur d'une batterie peut être empêchée, il y a peu de dilatation d'une batterie, et il y a peu de déformation même après un impact externe.
PCT/KR2014/010399 2013-10-31 2014-10-31 Ensemble électrode à pliage d'empilement WO2015065127A1 (fr)

Priority Applications (2)

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US14/762,409 US9484593B2 (en) 2013-10-31 2014-10-31 Stack-folding type electrode assembly
CN201480037483.0A CN105393399B (zh) 2013-10-31 2014-10-31 堆叠‑折叠型电极组件

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KR10-2013-0131584 2013-10-31
KR1020130131584A KR101676406B1 (ko) 2013-10-31 2013-10-31 스택-폴딩형 전극 조립체

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KR101676406B1 (ko) 2016-11-15
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KR20150050131A (ko) 2015-05-08
US9484593B2 (en) 2016-11-01

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